Search

Alkylamines are important precursors in secondary aerosol formation in the boreal forest atmosphere. To better understand the behaviour and sources of two alkylamines, dimethylamine (DMA) and diethylamine (DEA), we estimated the magnitudes of soil-atmosphere fluxes of DMA and DEA using a gradient-diffusion approximation based on measured concentrations in soil solution and in the canopy air space. To compute the amine fluxes, we first estimated the soil air space concentration from the measured soil solution amine concentration using soil physical (temperature, soil water content) and chemical (pH) state variables. Then, we used the resistance analogy to account for gas transport mechanisms in the soil, in soil boundary layer and in the canopy air space. The resulting flux estimates revealed that the boreal forest soil with a typical long-term mean pH 5.3 is a possible source of DMA (170 ± 51 nmol m-2 d-1) and a sink of DEA (-1.2 ± 1.2 nmol m-2 d-1). We also investigated the potential role of fungi as a reservoir for alkylamines in boreal forest soil. We found high DMA and DEA concentrations both in fungal hyphae collected from field humus samples and in fungal pure cultures. The highest DMA and DEA concentrations were found in fungal strains belonging to decay and ectomycorrhizal fungal groups, indicating that boreal forest soil, and in particular, fungal biomass may be an important reservoir for these alkylamines. [ABSTRACT FROM AUTHOR]

Aerosol formation from biogenic and anthropogenic precursor trace gases in continental background areas affects climate via altering the amount of available cloud condensation nuclei. Significant uncertainty still exists regarding the agents controlling the formation of aerosol nanoparticles. We have performed experiments in the Jülich plant-atmosphere simulation chamber with instrumentation for the detection of sulfuric acid and nanoparticles, and present the first simultaneous chamber observations of nanoparticles, sulfuric acid, and realistic levels and mixtures of biogenic volatile compounds (BVOCs). We present direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We directly measured particle formation rates separately from particle growth rates. From this, we established that in our experiments, the formation rate was proportional to the product of sulfuric acid and biogenic VOC emission strength. The formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid. The growth rate of nanoparticles immediately after birth was best correlated with estimated products resulting from BVOC ozonolysis. [ABSTRACT FROM AUTHOR]

The concentrations of neutral and charged sub-3 nm clusters and their connection to new particle formation (NPF) were investigated during the PEGASOS campaign (7 June-9 July 2012) at the San Pietro Capofiume measurement station in the Po Valley, Italy. Continuous high concentrations of sub-3 nm clusters were detected during the measurement period, although the condensation sink was relatively high (median value 1.1 × 10-2 s-1). The median cluster concentrations were 2140 and 7980 cm-3 in the size bins of 1.5-1.8 nm and 1.8-3 nm, and the majority of them were electrically neutral. NPF events were observed during the measurement period frequently, on 86% of the days. The median growth rates of clusters during the events were 4.3, 6.0 and 7.2 nm h-1 in the size ranges of 1.5-3, 3-7 and 7-20 nm. The median formation rate of 1.6 nm clusters was high, 45 cm-3 s-1, and it exceeded the median formation rate of 2 nm clusters by one order of magnitude. The ion-induced nucleation fraction was low; the median values were 0.7% at 1.6 nm and 3.0% at 2 nm. On NPF event days the neutral cluster concentration had a maximum around 9 a.m. (local winter time), which was absent on a non-event day. The increase in the cluster concentrations in the morning coincided with the increase in the boundary layer height. At the same time radiation and temperature increased and RH and condensation sink decreased. The concentration of neutral clusters was observed to have apositive correlation with sulfuric acid proxy, indicating the significance of sulfuric acid for the cluster formation in San Pietro Capofiume. The condensation sink had anegative correlation with the concentration of charged clusters but no clear relation to the neutral cluster concentration. This finding, together with back-trajectory analysis, suggests that the precursor vapors of the clusters and background aerosol particles, acting as their sink, have possibly originated from the same sources, including e.g. power plants and industrial areas in the Po Valley. [ABSTRACT FROM AUTHOR]

Air ion concentrations influence new particle formation and consequently the global aerosol as potential cloud condensation nuclei. We aimed to evaluate air ion concentrations and characteristics of new particle formation events (NPF) in the megacity of Paris, France, within the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric Pollution and climate effects, and Integrated tools for assessment and mitigation) project. We measured air ion number size distributions (0.8-42 nm) with an air ion spectrometer and fine particle number concentrations (> 6 nm) with a twin differential mobility particle sizer in an urban site of Paris between 26 June 2009 and 4 October 2010. Air ions were size classified as small (0.8- 2 nm), intermediate (2-7 nm), and large (7-20 nm). The median concentrations of small and large ions were 670 and 680 cm-3, respectively, (sum of positive and negative polarities), whereas the median concentration of intermediate ions was only 20 cm-3, as these ions were mostly present during new particle formation bursts, i.e. when gas-to-particle conversion produced fresh aerosol particles from gas phase precursors. During peaks in traffic-related particle number, the concentrations of small and intermediate ions decreased, whereas the concentrations of large ions increased. Seasonal variations affected the ion population differently, with respect to their size and polarity. NPF was observed in 13% of the days, being most frequent in spring and late summer (April, May, July, and August). The results also suggest that NPF was favoured on the weekends in comparison to workdays, likely due to the lower levels of condensation sinks in the mornings of weekends (CS weekdays 09:00: 18-10-3 s-1; CS weekend 09:00: 8-10-3 s-1/. The median growth rates (GR) of ions during the NPF events varied between 3 and 7 nm h-1, increasing with the ion size and being higher on workdays than on weekends for intermediate and large ions. The median GR of small ions on the other hand were rather similar on workdays and weekends. In general, NPF bursts changed the diurnal cycle of particle number as well as intermediate and large ions by causing an extra peak between 09:00 and 14:00. On average, during the NPF bursts the concentrations of intermediate ions were 8.5-10 times higher than on NPF non-event days, depending on the polarity, and the concentrations of large ions and particles were 1.5-1.8 and 1.2 times higher, respectively. Because the median concentrations of intermediate ions were considerably higher on NPF event days in comparison to NPF nonevent days, the results indicate that intermediate ion concentrations could be used as an indication for NPF in Paris. The results suggest that NPF was a source of ions and aerosol particles in Paris and therefore contributed to both air quality degradation and climatic effects, especially in the spring and summer. [ABSTRACT FROM AUTHOR]

The Pan-Eurasian Experiment (PEEX) is a multidisciplinary, multiscale and multicomponent research, research infrastructure and capacity-building program. PEEX has originated from a bottom-up approach by the science communities and is aiming at resolving the major uncertainties in Earth system science and global sustainability issues concerning the Arctic and boreal pan-Eurasian regions, as well as China. The vision of PEEX is to solve interlinked, global grand challenges influencing human well-being and societies in northern Eurasia and China. Such challenges include climate change; air quality; biodiversity loss; urbanization; chemicalization; food and freshwater availability; energy production; and use of natural resources by mining, industry, energy production and transport sectors. Our approach is integrative and supra-disciplinary, recognizing the important role of the Arctic and boreal ecosystems in the Earth system. The PEEX vision includes establishing and maintaining long-term, coherent and coordinated research activities as well as continuous, comprehensive research and educational infrastructure and related capacitybuilding across the PEEX domain. In this paper we present the PEEX structure and summarize its motivation, objectives and future outlook. [ABSTRACT FROM AUTHOR]

The oxidation of biogenic volatile organic compounds (BVOCs) gives a range of products, from semivolatile to extremely low-volatility compounds. To treat the interaction of these secondary organic vapours with the particle phase, global aerosol microphysics models generally use either a thermodynamic partitioning approach (assuming instant equilibrium between semi-volatile oxidation products and the particle phase) or a kinetic approach (accounting for the size dependence of condensation). We show that model treatment of the partitioning of biogenic organic vapours into the particle phase, and consequent distribution of material across the size distribution, controls the magnitude of the first aerosol indirect effect (AIE) due to biogenic secondary organic aerosol (SOA). With a kinetic partitioning approach, SOA is distributed according to the existing condensation sink, enhancing the growth of the smallest particles, i.e. those in the nucleation mode. This process tends to increase cloud droplet number concentrations in the presence of biogenic SOA. By contrast, an approach that distributes SOA according to pre-existing organic mass restricts the growth of the smallest particles, limiting the number that are able to form cloud droplets. With an organically mediated new particle formation mechanism, applying a mass-based rather than a kinetic approach to partitioning reduces our calculated global mean AIE due to biogenic SOA by 24%. Our results suggest that the mechanisms driving organic partitioning need to be fully understood in order to accurately describe the climatic effects of SOA. [ABSTRACT FROM AUTHOR]

Aerosol particles play important roles in regional air quality and global climate change. In this study, we analyzed 2 years (2011-2013) of measurements of submicron particles (6-800 nm) at a suburban site in the western Yangtze River Delta (YRD) of eastern China. The number concentrations (NCs) of particles in the nucleation, Aitken and accumulation modes were 5300±5500, 8000±4400, 5800±3200 cm-3, respectively. The NCs of total particles are comparable to those at urban/suburban sites in other Chinese megacities, such as Beijing, but about 10 times higher than in the remote western China. Long-range and regional transport largely influenced number concentrations and size distributions of submicron particles. The highest and lowest accumulation-mode particle number concentrations were observed in air masses from the YRD and coastal regions, respectively. Continental air masses from inland brought the highest concentrations of nucleation-mode particles. New particle formation (NPF) events, apparent in 44% of the effective measurement days, occurred frequently in all the seasons except winter. The frequency of NPF in spring, summer and autumn is much higher than other measurement sites in China. Sulfuric acid was found to be the main driver of NPF events. The particle formation rate was the highest in spring (3.6±2.4 cm-3 s-1/, whereas the particle growth rate had the highest values in summer (12.8±4.4 nm h-1/. The formation rate was typically high in relatively clean air masses, whereas the growth rate tended to be high in the polluted YRD air masses. The frequency of NPF events and the particle growth rates showed a strong year-to-year difference. In the summer of 2013, associated with a multi-week heat wave and strong photochemical processes, NPF events occurred with larger frequency and higher growth rates compared with the same period in 2012. The difference in the location and strength of the subtropical high pressure system, which influences the air mass transport pathways and solar radiation, seems to be the cause for year-to-year differences. This study reports, up to now, the longest continuous measurement records of submicron particles in eastern China and helps to achieve a comprehensive understanding of the main factors controlling the seasonal and year-to-year variation of the aerosol size distribution and NPF in this region. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) occurs frequently in the global atmosphere. During recent years, detailed laboratory experiments combined with intensive field observations in different locations have provided insights into the vapours responsible for the initial formation of particles and their subsequent growth. In this regard, the importance of sulfuric acid, stabilizing bases such as ammonia and amines as well as extremely low volatile organics, have been proposed. The instrumentation to observe freshly formed aerosol particles has developed to a stage where the instruments can be implemented as part of airborne platforms, such as aircrafts or a Zeppelin-type airship. Flight measurements are technically more demanding and require a greater detail of planning than field studies at the ground level. The high cost of flight hours, limited time available during a single research flight for the measurements, and different instrument payloads in Zeppelin airship for various flight missions demanded an analysis tool that would forecast whether or not there is a good chance for an NPF event. Here we present a methodology to forecast NPF event probability at the SMEAR II site in Hyytiälä, Finland. This methodology was used to optimize flight hours during the PEGASOS (Pan-European Gas Aerosol Climate Interaction Study)--Zeppelin Northern mission in May--June 2013. Based on the existing knowledge, we derived a method for estimating the nucleation probability that utilizes forecast air mass trajectories, weather forecasts, and air quality model predictions.With the forecast tool we were able to predict the occurrence of NPF events for the next day with more than 90% success rate (10 out of 11 NPF event days correctly predicted). To our knowledge, no similar forecasts of NPF occurrence have been developed for other sites. This method of forecasting NPF occurrence could be applied also at other locations, provided that long-term observations of conditions favouring particle formation are available. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) has been investigated intensively during the last two decades because of its influence on aerosol population and the possible contribution to cloud condensation nuclei. However, intensive measurements and modelling activities on this topic in urban metropolitans in China with frequently high pollution episodes are still very limited. This study provides results from a comprehensive modelling study on the occurrence of new particle formation events in the western part of the Yangtze River Delta region (YRD), China. The comprehensive modelling system, which combines regional chemical transport model WRF-Chem (the Weather Research and Forecasting model coupled with Chemistry) and the sectional box model MALTE-BOX (the model to predict new aerosol formation in the lower troposphere), was shown to be capable of simulating atmospheric nucleation and subsequent growth. Here we present a detailed discussion of three typical NPF days, during which the measured air masses were notably influenced by either anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. Overall, simulated NPF events were generally in good agreement with the corresponding measurements, enabling us to get further insights into NPF processes in the YRD region. Based on the simulations, we conclude that besides gas-phase sulphuric acid, biogenic organic compounds, particularly monoterpenes, play an essential role in condensational growth of newly formed clusters and probably also in the particle formation process through their low volatile oxidation products. Although some uncertainties remain in this modelling system, this method provides a possibility to better understand the NPF processes. [ABSTRACT FROM AUTHOR]

Disproportional warming in the northern high latitudes, and large carbon stocks in boreal and (sub)arctic ecosystems have raised concerns as to whether substantial positive climate feedbacks from biogeochemical process responses should be expected. Such feedbacks occur if increasing temperatures lead to e.g. a net release of CO2 or CH4. However, temperature-enhanced emissions of biogenic volatile organic compounds (BVOC) have been shown to contribute to the growth of secondary organic aerosol (SOA) which is known to have a negative radiative climate effect. Combining measurements in Eastern Siberia with model-based estimates of vegetation and permafrost dynamics, BVOC emissions and aerosol growth, we assess here possible future changes in ecosystem CO2 balance and BVOC-SOA interactions, and discuss these changes in terms of possible climate effects. On global level, both are very small but when concentrating on Siberia and the northern hemisphere the negative forcing from changed aerosol direct and indirect effects become notable - even though the associated temperature response would not necessarily follow a similar spatial pattern. While our analysis does not include other important processes that are of relevance for the climate system, the CO2 and BVOC-SOA interplay used serves as an example of the complexity of the interactions between emissions and vegetation dynamics that underlie individual terrestrial feedbacks and highlights the importance of addressing ecosystem-climate feedbacks in consistent, process-based model frameworks. [ABSTRACT FROM AUTHOR]

Measurements of the hygroscopicity of 15-145 nm particles in a boreal forest environment were conducted using two Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) systems during the Pan-European Gas-Aerosols-climate interaction Study (PEGASOS) campaign in spring 2013. Measurements of the chemical composition of non-size segregated particles were also performed using a high-resolution aerosol mass spectrometer (HR-AMS) in parallel with hygroscopicity measurements. On average, the hygroscopic growth factor (HGF) of particles was observed to increase from the morning until afternoon. In case of accumulation mode particles, the main reasons for this behavior were increases in the ratio of sulfate to organic matter and oxidation level (OC : ratio) of the organic matter in the particle phase. Using an OC : dependent hygroscopic growth factor of organic matter (HGForg), fitted using the inverse Zdanovskii-Stokes-Robinson (ZSR) mixing rule, clearly improved the agreement between measured HGF and that predicted based on HR-AMS composition data. Besides organic oxidation level, the influence of inorganic species was tested when using the ZSR mixing rule to estimate the hygroscopic growth factor of organics in the aerosols. While accumulation and Aitken mode particles were predicted fairly well by the bulk aerosol composition data, the hygroscopicity of nucleation mode particles showed little correlation. However, we observed them to be more sensitive to the gas phase concentration of condensable vapors: the more sulfuric acid in the gas phase, the more hygroscopic the nucleation mode particles were. No clear dependence was found between the extremely low-volatility organics concentration (ELVOC) and the HGF of particles of any size. [ABSTRACT FROM AUTHOR]

During the CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) campaign, the interaction between aerosol particles and cloud microphysical properties was investigated in detail, which also includes the influence of clouds on the aerosol formation. During two intensive campaigns in 2010 and 2011, helicopter-borne measurement flights were performed to investigate the thermodynamic, turbulent, microphysical, and radiative properties of trade-wind cumuli over Barbados. During these flights, 91 cases with increased aerosol particle number concentrations near clouds were detected. The majority of these cases are also correlated with enhanced irradiance in the ultraviolet (UV) spectral wavelength range. This enhancement reaches values up to a factor of 3.3 greater compared to background values. Thus, cloud boundaries provide a perfect environment for the production of precursor gases for new particle formation. Another feature of cloud edges is an increased turbulence, which may also enhance nucleation and particle growth. The observed events have a mean length of 100 m, corresponding to a lifetime of less than 300 s. This implies that particles with diameters of at least 7 nm grew several nanometers per minute, which corresponds to the upper end of values in the literature (Kulmala et al., 2004). Such high values cannot be explained by sulfuric acid alone; thus extremely low volatility organic compounds (ELVOCs) are probably involved here. [ABSTRACT FROM AUTHOR]

The Pan-Eurasian Experiment (PEEX) is a multi-disciplinary, multi-scale and multicomponent research, research infrastructure and capacity building program. PEEX has originated from a bottom-up approach by the science communities, and is aiming at resolving the major uncertainties in Earth System Science and global sustainability issues concerning the Arctic and boreal Pan-Eurasian regions, as well as China. The vision of PEEX is to solve interlinked global grand challenges influencing human wellbeing and societies in northern Eurasia and China. Such challenges include climate change, air quality, biodiversity loss, urbanization, chemicalization, food and fresh water availability, energy production and use of natural resources by mining, industry, energy production and transport sectors. Our approach is integrative and supra-disciplinary, recognizing the important role of the Arctic and boreal ecosystems in the Earth system. The PEEX vision includes establishing and maintaining long-term, coherent and coordinated research activities as well as continuous, comprehensive research and educational infrastructures and related capacity building across the PEEX domain. In this paper we present the PEEX structure, summarize its motivation, objectives and future outlook. [ABSTRACT FROM AUTHOR]

Ambient particle number size distributions were measured in Paris, France, during summer (1-31 July 2009) and winter (15 January to 15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation (MEGAPOLI) project. New particle formation (NPF) was observed only during summer on approximately 50% of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10-3 s-1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from the Paris center during summer. The number concentration of particles with diameters exceeding 2.5 nm measured on the surface at the Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm-3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer, one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of 3 when it was downwind of Paris. [ABSTRACT FROM AUTHOR]

The global environment is changing rapidly due to anthropogenic emissions and actions. Such activities modify aerosol and greenhouse gas concentrations in the atmosphere, leading to regional and global climate change and affecting e.g. food and fresh-water security, sustainable use of natural resources and even demography. Here we present a conceptual design of a global, hierarchical observation network that can provide tools and increased understanding to tackle the inter-connected environmental and societal challenges that we will face in the coming decades. The philosophy behind the conceptual design relies on physical conservation laws of mass, energy and momentum, as well as on concentration gradients that act as driving forces for the atmosphere-biosphere exchange. The network is composed of standard, flux/advanced and flagship stations, each of which having specific and identified tasks. Each ecosystem type on the globe has its own characteristic features that have to be taken into consideration. The hierarchical network as a whole is able to tackle problems related to large spatial scales, heterogeneity of ecosystems and their complexity. The most comprehensive observations are envisioned to occur in flag ship stations, with which the process-level understanding can be expanded to continental and global scales together with advanced data analysis, earth system modelling and satellite remote sensing. The denser network of the flux and standard stations allow application and up-scaling of the results obtained from flag ship stations to the global level. [ABSTRACT FROM AUTHOR]

While cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is thought to be frequent throughout the continental boundary layers, few studies on this phenomenon in marine air exist. Here, based on simultaneous measurement of particle number size distributions, CCN properties and aerosol chemical composition, we present the first direct evidence on CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles to CCN sizes in this environment during the summertime. Sub-100 nm particles were found to be substantially less hygroscopic than larger particles during the period with active NPF and growth (the value of κ was lower by 0.2-0.4 for 60 nm particles compared with 120 nm particles), probably due to enrichment of organic material in the sub-100 nm size range. The aerosol hygroscopicity tended to be at minimum just before the noon and at maximum in the afternoon, which was very likely due to the higher sulfate-to-organic ratios and higher degree of oxidation of the organic material during the afternoon. Simultaneous with the formation of new particles during daytime, particles formed during the previous day or even earlier were growing into the size range relevant to cloud droplet activation, and the particles formed in the atmosphere were possibly mixed with long-range-transported particles. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) is an important atmospheric phenomenon. During an NPF event, particles first form by nucleation and then grow further in size. The growth step is crucial because it controls the number of particles that can become cloud condensation nuclei. Among various physical and chemical processes contributing to particle growth, condensation by organic vapors has been suggested as important. In order to better understand the influence of biogenic emissions on particle growth, we carried out modeling studies of NPF events during the BEACHON-ROCS (Bio- hydro-atmosphere interactions of Energy, Aerosol, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Organic Carbon Study) campaign at Manitou Experimental Forest Observatory in Colorado, USA. The site is representative of the semi-arid western USA. With the latest Criegee intermediate reaction rates implemented in the chemistry scheme, the model underestimates sulfuric acid concentration by 50%, suggesting either missing sources of atmospheric sulfuric acid or an overestimated sink term. The results emphasize the contribution from biogenic volatile organic compound emissions to particle growth by demonstrating the effects of the oxidation products of monoterpenes and 2-Methyl-3-buten- 2-ol (MBO). Monoterpene oxidation products are shown to influence the nighttime particle loadings significantly, while their concentrations are insufficient to grow the particles during the day. The growth of ultrafine particles in the daytime appears to be closely related to the OH oxidation products of MBO. [ABSTRACT FROM AUTHOR]

Measuring sub-3nm particles outside of controlled laboratory conditions is a challenging task, as many of the instruments are operated at their limits and are subjected to changing ambient conditions. In this study, we advance the current understanding on the operation of Airmodus A11 nano Condensation Nucleus Counter (nCNC), which consists of a A10 Particle Size Magnifier (PSM) and A20 condensation particle counter (CPC). We explore the effect of the inlet line pressure on the measured particle concentration. We identify two different regions inside the instrument where supersaturation of working fluid can take place. We show the possibility of varying the cut-off of the instrument from 1 to 6 nm, a wider size range than the one usually covered by the PSM. We also present a new inlet system, which allows automated measurements of the background, minimizes the diffusion losses in the sampling line and is equipped with an electrostatic filter to remove ions. Finally, our view of the guidelines for optimal use of the Airmodus nCNC are provided. [ABSTRACT FROM AUTHOR]

Over the last few years, several condensation particle counters (CPCs) capable of measuring in the sub-3 nm size range have been developed. Here we study the performance of CPCs based on diethylene glycol (DEG) at different temperatures during Cosmics Leaving OUtdoor Droplets (CLOUD) measurements at CERN. The data shown here are the first set of verification measurements for sub-3 nm CPCs under upper tropospheric temperatures using atmospherically relevant aerosol particles. To put the results in perspective we calibrated the DEG-CPC at room temperature, resulting in a cut-off diameter of 1.4 nm. All diameters refer to mobility equivalent diameters in this paper. At upper tropospheric temperatures ranging from 246.15 K to 207.15 K, we found cut-off sizes relative to a particle size magnifier in the range of 2.5 to 2.8 nm. Due to low number concentration after size classification, the cut-off diameters have a high uncertainty (±0.3 nm) associated with them. Operating two laminar flow DEG-CPCs with different cut-off sizes together with other aerosol instruments, we looked at the growth rates of aerosol population in the CLOUD chamber for particles smaller than 10 nm at different temperatures. A more consistent picture emerged when we normalized the growth rates to a fixed gas-phase sulfuric acid concentration. All of the instruments detected larger growth rates at lower temperatures, and the observed growth rates decreased as a function of temperature, showing a similar trend for all instruments. The theoretical calculations had a similar but much smaller temperature dependency. [ABSTRACT FROM AUTHOR]

Proxies for estimating nucleation mode number concentrations and further simplification for their use with satellite data have been presented in Kulmala et al. (2011). In this paper we discuss the underlying assumptions for these simplifications and evaluate the resulting proxies over an area in South Africa based on a comparison with a suite of ground-based measurements available from four different stations. The proxies are formulated in terms of sources (concentrations of precursor gases (NO2 and SO2) and UVB radiation intensity near the surface) and a sink term related to removal of the precursor gases due to condensation on pre-existing aerosols. A-Train satellite data are used as input to compute proxies. Both the input data and the resulting proxies are compared with those obtained from ground-based measurements. In particular, a detailed study is presented on the substitution of the local condensation sink (CS) with satellite aerosol optical depth (AOD), which is a columnintegrated parameter. One of the main factors affecting the disagreement between CS and AOD is the presence of elevated aerosol layers. Overall, the correlation between proxies calculated from the in situ data and observed nucleation mode particle number concentrations (Nnuc) remained low. At the time of the satellite overpass (13:00-14:00 LT) the highest correlation is observed for SO2/CS (R² D 0:2). However, when the proxies are calculated using satellite data, only NO2/AOD showed some correlation with Nnuc (R² D 0:2). This can be explained by the relatively high uncertainties related especially to the satellite SO2 columns and by the positive correlation that is observed between the ground-based SO2 and NO2 concentrations. In fact, results show that the satellite NO2 columns compare better with in situ SO2 concentration than the satellite SO2 column. Despite the high uncertainties related to the proxies calculated using satellite data, the proxies calculated from the in situ data did not better predict Nnuc. Hence, overall improvements in the formulation of the proxies are needed. [ABSTRACT FROM AUTHOR]

Aerosol particles play important roles in regional air quality and global climate change. In this study, we analyzed two-year (2011-2013) of measurements of submicron particles (6-800 nm) at a suburban site in western Yangtze River delta (YRD) of East China. The number concentrations (NCs) of particles in the nucleation, Aitken and accumulation modes were 5300 ± 5500, 8000 ± 4400, 5800 ± 3200 cm-3, respectively. Number concentrations and size distributions of submicron particles were also influenced by long-range and regional transport of air masses. The highest and lowest accumulation mode particle number concentrations were observed in air masses from YRD and coastal region, respectively. Continental air masses from inland had the highest concentrations of nucleation mode particles. New particle formation (NPF) events, apparent in 44% of the effective measurement days, occurred frequently in all the seasons except winter. Radiation and pre-existing particles were found to be the main factors influencing the occurrence of NPF events. The particle formation rate was the highest in spring (3.6 ± 2.4 cm-3 s-1), whereas the particle growth rate had the highest values in summer (12.8 ± 4.4nmh-1). The formation rate was typically high in relatively clean air masses, whereas the growth rate tended to be high in the polluted YRD air masses. The frequency of NPF events and the growth rate showed a strong year-to-year difference. In the summer of 2013, associated with a multi-week heat wave and photochemical pollution, NPF events occurred more frequently and the growth rate was much higher than in the same period of 2012. The difference in the location and strength of sub-tropical High, which influences the air mass transport pathways and solar radiation, seems to be the driving cause for year-to-year differences. This study reported the longest continuous measurement records of submicron particles in the East China and gained a comprehensive understanding of the main factors controlling the seasonal and year-to-year variation of the aerosol size distribution and NPF in the East China. The work highlights the importance and need for long-term measurements in understanding the atmosphere system and the impact by human activities. [ABSTRACT FROM AUTHOR]

While Cloud Condensation Nuclei (CCN) production associated with atmospheric new particle formation (NPF) is thought to be frequent throughout the continental boundary layers, few studies on this phenomenon in marine air exist. Here, based on simultaneous measurement of particle number size distributions, CCN properties and aerosol chemical composition, we present the first direct evidence on CCN production resulting from NPF in the Eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles to CCN sizes in this environment during the summertime. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the period with active NPF and growth (0.2-0.4 lower α between the 60 and 120nm particles), probably due to enrichment of organic material in the sub-100nm size range. The aerosol hygroscopicity tended to be at minimum just before the noon and at maximum in afternoon, which was very likely due to the higher sulfate to organic ratios and higher degree of oxidation of the organic material during the afternoon. Simultaneously to the formation of new particles during daytime, particles formed in the previous day or even earlier were growing into the size range relevant to cloud droplet activation, and the particles formed in the atmosphere were possibly mixed with long-range transported particles. [ABSTRACT FROM AUTHOR]

Using the 1-D atmospheric chemistry transport model SOSAA, we have investigated the atmospheric reactivity of a boreal forest ecosystem during the HUMPPACOPEC- 10 campaign (summer 2010, at SMEAR II in southern Finland). For the very first time, we present vertically resolved model simulations of the NO3 and O3 reactivity (R) together with the modelled and measured reactivity of OH. We find that OH is the most reactive oxidant (R ~3 s-1) followed by NO3 (R ~0:07 s-1) and O3 (R ~2✕10-5 s-1). The missing OH reactivity was found to be large in accordance with measurements (~65%) as would be expected from the chemical subset described in the model. The accounted OH radical sinks were inorganic compounds (~ 41%, mainly due to reaction with CO), emitted monoterpenes (~14%) and oxidised biogenic volatile organic compounds (~44%). The missing reactivity is expected to be due to unknown biogenic volatile organic compounds and their photoproducts, indicating that the true main sink of OH is not expected to be inorganic compounds. The NO3 radical was found to react mainly with primary emitted monoterpenes (~60%) and inorganic compounds (~37%, including NO2). NO2 is, however, only a temporary sink of NO3 under the conditions of the campaign (with typical temperatures of 20-25 °C) and does not affect the NO3 concentration. We discuss the difference between instantaneous and steadystate reactivity and present the first boreal forest steady-state lifetime of NO3 (113 s). O3 almost exclusively reacts with inorganic compounds (~91%, mainly NO, but also NO2 during night) and less with primary emitted sesquiterpenes (~6%) and monoterpenes (~ 3%). When considering the concentration of the oxidants investigated, we find that OH is the oxidant that is capable of removing organic compounds at a faster rate during daytime, whereas NO3 can remove organic molecules at a faster rate during night-time. O3 competes with OH and NO3 during a short period of time in the early morning (around 5 a.m. local time) and in the evening (around 7-8 p.m.). As part of this study, we developed a simple empirical parameterisation for conversion of measured spectral irradiance into actinic flux. Further, the meteorological conditions were evaluated using radiosonde observations and ground-based measurements. The overall vertical structure of the boundary layer is discussed, together with validation of the surface energy balance and turbulent fluxes. The sensible heat and momentum fluxes above the canopy were on average overestimated, while the latent heat flux was underestimated. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) is an important atmospheric phenomenon. During a NPF event, molecular clusters first form by nucleation and then grow further by condensation of vapors. The growth step is crucial because it controls the number of particles that can become cloud condensation nuclei. In order to better understand the influence of biogenic emissions on particle growth, we carried out modeling studies of NPF events during the BEACHON-ROCS campaign at Manitou Experimental Forest Observatory in Colorado, USA. The site is representative of the semi-arid Western US. The implemented chemistry scheme with the latest Criegee intermediates reaction rates under estimates sulfuric acid concentration by 50%, suggesting missing atmospheric sulfuric acid sources. The results emphasize the contribution from biogenic volatile organic compound emissions to particle growth by demonstrating the effects of the oxidation products of monoterpenes and 2-Methyl-3-buten-2-ol (MBO). Monoterpene oxidation products are shown to influence the nighttime particle loadings significantly while their concentrations are insufficient to grow the particles during the day. The growth of ultrafine particles in daytime appears to be closely related to the OH oxidation products of MBO. [ABSTRACT FROM AUTHOR]

The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular at high altitude, where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around highaltitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to ~ 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report day-time concentrations of charged and neutral clusters (1 to 2.5 nm mobility diameter) recorded at the interface between the boundary layer (BL) and the FT as well as in the FT at the altitude site of Puy de Dôme (1465 ma.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the FT, and especially at the interface between the BL and the FT, the formation of 1.5 nm neutral clusters significantly exceeds the one of ionic clusters during NPF events, clearly indicating that they dominate in the nucleation process. We also observe that the total cluster concentration significantly increases during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. During the studied period, the nucleation process does not seem to be sulfuric acid-limited and could be promoted by the transport of pollutants to the upper troposphere, coupled with low temperatures. [ABSTRACT FROM AUTHOR]

Sulfuric acid is known to be a key component for atmospheric nucleation. Precise determination of sulfuricacid concentration is a crucial factor for prediction of nucleation rates and subsequent growth. In our study, we have noticed a substantial discrepancy between sulfuricacid monomer concentrations and total-sulfate concentrations measured from the same source of sulfuric-acid vapor. The discrepancy of about 1-2 orders of magnitude was found with similar particle-formation rates. To investigate this discrepancy, and its effect on nucleation, a method of thermally controlled saturator filled with pure sulfuric acid (97%wt.) for production of sulfuric-acid vapor is applied and rigorously tested. The saturator provided an independent vapor-production method, compared to our previous method of the furnace (Brus et al., 2010, 2011), to find out if the discrepancy is caused by the production method itself. The saturator was used in a H2SO4-H2O nucleation experiment, using a laminar flow tube to check reproducibility of the nucleation results with the saturator method, compared to the furnace. Two independent methods of mass spectrometry and online ion chromatography were used for detecting sulfuric-acid or sulfate concentrations. Measured sulfuricacid or total-sulfate concentrations are compared to theoretical predictions calculated using vapor pressure and a mixing law. The calculated prediction of sulfuric-acid concentrations agrees very well with the measured values when total sulfate is considered. Sulfuric-acid monomer concentration was found to be about 2 orders of magnitude lower than theoretical predictions, but with a temperature dependency similar to the predictions and the results obtained with the ion-chromatograph method. Formation rates are reproducible when compared to our previous results with both sulfuric-acid or total-sulfate detection and sulfuric-acid production methods separately, removing any doubts that the vapor-production method would cause the discrepancy. Possible reasons for the discrepancy are discussed and some suggestions include that the missing sulfuric acid is in clusters, formed with contaminants found in most laboratory experiments. One-to-two-order-of-magnitude higher sulfuric-acid concentrations (measured as total sulfate in this study) would contribute to a higher fraction of particle growth rate than assumed from the measurements by mass spectrometers (i.e. sulfuric-acid monomer). However, the observed growth rates by sulfate-containing vapor in this study does not directly imply a similar situation in the field, where sources of sulfate are much more diverse. [ABSTRACT FROM AUTHOR]

Ambient particle number size distributions were measured in Paris, France during summer (1-31 July 2009) and winter (15 January-15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the MEGAPOLI project. New particle formation (NPF) was observed only during summer at approximately 50% of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10-3 s-1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from Paris center during summer. The number concentration of particles with diameter exceeding 2.5 nm measured on the surface at Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm-3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of three when it was downwind of Paris. [ABSTRACT FROM AUTHOR]

Particle size distributions in the range of 1.34-615 nm were recorded from 25 November 2013 to 25 January 2014 in urban Shanghai, using a combination of one nano condensation nucleus counter system, one nano scanning mobility particle sizer (SMPS), and one long-SMPS. Measurements of sulfur dioxide by an SO2 analyzer with pulsed UV fluorescence technique allowed calculation of sulfuric acid proxy. In addition, concentrations of ammonia were recorded with a differential optical absorption spectroscopy. During this 62-day campaign, 13 new particle formation (NPF) events were identified with strong bursts of sub-3 nm particles and subsequent fast growth of newly formed particles. The observed nucleation rate (J1.34), formation rate of 3 nm particles (J3), and condensation sink were 112.4-271.0 cm-3 s-1, 2.3-19.2 cm-3 s-1, and 0.030-0.10 s-1, respectively. Subsequent cluster/nanoparticle growth (GR) showed a clear size dependence, with average values of GR1.35~1.39, GR1.39~1.46, GR1.46~1.70, GR1.70~2.39, GR2.39~7, and GR7~20 being 1.6 ± 1.0, 1.4±2.2, 7.2±7.1, 9.0±11.4, 10.9±9.8, and 11.4± 9.7 nm h-1, respectively. Correlation between nucleation rate (J1.34) and sulfuric acid proxy indicates that nucleation rate J1.34 was proportional to a 0.65±0.28 power of sulfuric acid proxy, indicating that the nucleation of particles can be explained by the activation theory. Correlation between nucleation rate (J1.34) and gas-phase ammonia suggests that ammonia was associated with NPF events. The calculated sulfuric acid proxy was sufficient to explain the subsequent growth of 1.34-3 nm particles, but its contribution became smaller as the particle size grew. Qualitatively, NPF events in urban Shanghai likely occur on days with low levels of aerosol surface area, meaning the sulfuric acid proxy is only a valid predictor when aerosol surface area is low. [ABSTRACT FROM AUTHOR]

Nitrous acid (HONO) plays a key role in atmospheric chemistry by influencing the budget of hydroxyl radical (OH). In this study, a two-month measurement of HONO and related quantities were analyzed during a biomass burning season in 2012 at a suburban site in the western Yangtze River delta, eastern China. An overall high HONO concentration with the mean value of 0.76 ppbv (0.01 ppbv to 5.95 ppbv) was observed. During biomass burning (BB) periods, both HONO concentration and HONO/NO2 ratio were enhanced significantly (more than a factor of 2, p<0.01) compared with non-biomass burning (non-BB) periods. A correlation analysis showed that the HONO in BB plumes was more correlated with nitrogen dioxide (NO2) than that with potassium (a tracer of BB). Estimation by the method of potassium tracing suggests a maximum contribution of 17 ± 12% from BB emission to the observed HONO concentrations, and the other over 80% of the observed nighttime HONO concentrations during BB periods were secondarily produced by the heterogeneous conversion of NO2. The NO2-to-HONO conversion rate (CHONO) in BB plumes was almost twice as that in non-BB plumes (0.0062 hr-1 vs. 0.0032 hr-1). Given that the residence time of the BB air masses was lower than that of non-BB air masses, these results suggest BB aerosols have higher NO2 conversion potentials to form HONO than non-BB aerosols. A further analysis based on comparing the surface area at similar particle mass levels and HONO/NO2 ratios at similar surface area levels suggested larger specific surface areas and higher NO2 conversion efficiencies of BB aerosols. A mixed plume of BB and anthropogenic fossil fuel (FF) emissions was observed on 10 June with even higher HONO concentrations and HONO/NO2 ratios. The strong HONO production potential (high HONO/NO2 to PM2.5 ratio) was accompanied with a high sulfate concentration in this plume, suggesting a promotion of mixed aerosols to the HONO formation. In summary, our study suggests an important role of BB in atmospheric chemistry by affecting the HONO budget. This can be especially important in eastern China, where agricultural burning plumes are inevitably mixed with urban and industrial pollution. [ABSTRACT FROM AUTHOR]

This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the diurnal evolution of the meteorological and gas phase parameters involved. Atmospheric aerosol observations include Neutral cluster and Air Ion Spectrometer (NAIS) measurements at the research station Melpitz, East Germany between 2008 and 2011. Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter range 2-20 nm. To study the relationship with gaseous precursors, a proximity measure was calculated for the sulfuric acid concentration on the basis of a one month intensive measurement campaign in May 2008. A major result was that the number concentration of fresh produced neutral particles correlated significantly with the amount of sulfur dioxide available as a main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations, which also represent a recognised precursor of aerosol particle nucleation. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events, and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established with certainty. On the basis of observed diurnal cycles of aerosol, gas phase, and meteorological parameters near the ground, we conclude that particle formation is likely to be induced aloft, rather than near the ground. [ABSTRACT FROM AUTHOR]

The global potential for collecting usable water from dew on an artificial collector sheet was investigated by utilizing 34 years of meteorological reanalysis data as input to a dew formation model. Continental dew formation was found to be frequent and common, but daily yields were mostly below 0.1mm. Nevertheless, some water-stressed areas such as parts of the coastal regions of northern Africa and the Arabian Peninsula show potential for large-scale dew harvesting, as the yearly yield may reach up to 100 L m-2 for a commonly used polyethylene foil. Statistically significant trends were found in the data, indicating overall changes in dew yields of between ±10% over the investigated time period. [ABSTRACT FROM AUTHOR]

A satellite-based approach to derive the aerosol direct shortwave (SW) radiative effect (ADRE) was studied in an environment with highly variable aerosol conditions over eastern China from March to October 2009. The method is based on using coincident SW top-of-the-atmosphere (TOA) fluxes from the Clouds and the Earth's Radiant Energy System (CERES) and aerosol optical depths (AODs) from the MODerate Resolution Imaging Spectroradiometer (MODIS) to derive SW clear-sky ADRE. The estimate for the aerosolfree TOA flux (F0,TOA) is obtained by establishing linear regression between CERES SW TOA fluxes and MODIS AODs. A normalization procedure to a fixed solar zenith angle, Earth-Sun distance and atmospheric water vapor content was applied to the CERES fluxes prior to the linear fit against AOD to reduce the flux variation not related to aerosols. In the majority of the cases, the normalization increased positive correlation between observed SW TOA fluxes and AODs, and it decreased RMSE. The key question in the satellite-based approach is the accuracy of the estimated F0,TOA. Comparison with simulated F0,TOA showed that both the satellite method and the model produced qualitatively similar spatial patterns, but absolute values differed. In 58% of the cases the satellite-based F0,TOA was within ±10 Wm-2 of the modeled value (about 7-8% difference in flux values). Over bright surfaces, the satellite-based method tend to produce lower F0,TOA than the model. The satellitebased clear-sky estimates for median instantaneous and diurnally averaged ADRE over the study area were --8.8 Wm-2 and --5.1Wm--2, respectively. Over heavily industrialized areas, the cooling at TOA was 2 to more than 3 times the median value, and associated with high AODs (> 0.5). Especially during the summer months, positive ADREs were observed locally over dark surfaces. This was most probably a method artifact related to systematic change of aerosol type, sub-visual cloud contamination or both. [ABSTRACT FROM AUTHOR]

Aerosol formation from biogenic and anthropogenic precursor trace gases in continental background areas affects climate via altering the amount of available cloud condensation nuclei. Significant uncertainty still exists regarding the agents controlling the formation of aerosol nanoparticles. We have performed experiments in the Jülich Plant-Atmosphere Simulation Chamber with instrumentation for the detection of sulphuric acid and nanoparticles, and present the first simultaneous chamber observations of nanoparticles, sulphuric acid, and realistic levels and mixtures of biogenic volatile compounds (BVOC). We present direct laboratory observations of nanoparticle formation from sulphuric acid and realistic BVOC precursor vapor mixtures performed at atmospherically relevant concentration levels. We directly measured particle formation rates separately from particle growth rates. From this, we established that in our experiments, the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength. The formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulphuric acid. The growth rate of nanoparticles immediately after birth was best correlated with estimated products resulting from BVOC ozonolysis. [ABSTRACT FROM AUTHOR]

Using the 1D atmospheric chemistry-transport model SOSAA, we have investigated the atmospheric reactivity of a boreal forest ecosystem during the HUMPPA-COPEC-10 campaign (summer 2010, at SMEAR II in Southern Finland). For the very first time, we present vertically resolved model simulations of the NO3- and O3-reactivity (R) together with the modelled and measured reactivity of OH. We find that OH is the most reactive oxidant (R ~ 3 s-1) followed by NO3 (R ~ 0.07s-1) and O3 (R ~ 2 x10-5 s-1). The missing OH-reactivity was found to be large in accordance with measurements (~ 65%) as would be expected from the chemical subset described in the model. The accounted OH radical sinks were inorganic compounds (~ 41%, mainly due to reaction with CO), emitted monoterpenes (~ 14%) and oxidised biogenic volatile organic compounds (~ 44%). The missing reactivity is expected to be due to unknown biogenic volatile organic compounds and their photoproducts, indicating that the true main sink of OH is not expected to be inorganic compounds. The NO3 radical was found to react mainly with primary emitted monoterpenes (~ 60%) and inorganic compounds (~ 37%, including NO2). NO2 is, however, only a temporary sink of NO3 under the conditions of the campaign and does not affect the NO3 concentration. We discuss the difference between instantaneous and steady state reactivity and present the first boreal forest steady state lifetime of NO3 (113 s). O3 almost exclusively reacts with inorganic compounds (~ 91%, mainly NO, but also NO2 during night) and less with primary emitted sesquiterpenes (~ 6%) and monoterpenes (~ 3%). When considering the concentration of the oxidants investigated, we find that O3 is the oxidant that is capable of removing pollutants fastest. As part of this study, we developed a simple empirical parameterisation for conversion of measured spectral irradiance into actinic flux. Further, the meteorological conditions were evaluated using radiosonde observations and ground based measurements. The overall vertical structure of the boundary layer is discussed, together with validation of the surface energy balance and turbulent [ABSTRACT FROM AUTHOR]

Particle size distributions in the range of 1.34-615.3nm were recorded from 25 November 2013 to 25 January 2014 in urban Shanghai, using a combination of one nano Condensation Nucleus Counter system (nCNC), one nano-Scanning Mobility Particle Sizer (SMPS), and one long-SMPS. Measurements of sulfur dioxide by an SO2 analyzer with pulsed UV fluorescence technique allowed calculation of sulfuric acid proxy. In addition, concentrations of ammonia were recorded with a Differential Optical Absorption Spectroscopy (DOAS). During this 62-day campaign, 13 NPF events were identified with strong burst of sub-3nm particles and subsequent fast growth of newly formed particles. The observed nucleation rate (J1.34), formation rate of 3 nm particles (J3), and condensation sink (CS) were 112.4-271.0 cm-3 s-1, 2.3-19.2 cm-3 s-1, and 0.030- 0.10 s-1, respectively. Subsequent cluster/nanoparticle growth showed a clear size dependence, with average values of GR1.35~1.39(from the bin of 1.34-1.37nm to the bin of 1.37-1.41 nm), GR1.39~1.46 (from 1.37-1.41 to 1.41-1.52 nm), GR1.46~1.70 (from 1.41- 1.52 to 1.52-1.89 nm), GR1.70~2.39 (from 1.52-1.89 to 1.89-3.0 nm), GR2.39~7 (from 1.89-3.0 to 7 nm), and GR7~20 (from 7 to 20 nm) being 1.6±1.0, 1.4±2.2, 7.2±7.1, 9.0±11.4, 10.9±9.8, and 11.4±9.7nmh-1, respectively. Correlation between nucleation rate (J1.34) and sulfuric acid proxy indicates that nucleation rate J1.34 was proportional to a 0.64 power of sulfuric acid proxy. Correlation between nucleation rate (J1.34) and gas-phase ammonia suggests that ammonia was associated with NPF events. The calculated sulfuric acid proxy was sufficient to explain the subsequent growth of 1.34- 3nm particles, but insufficient for particles exceeding this size range. Qualitatively, NPF events in urban Shanghai likely occur on days with low levels of PM2.5. [ABSTRACT FROM AUTHOR]

Biogenic volatile organic compounds (BVOCs) are essential in atmospheric chemistry because of their chemical reactions that produce and destroy tropospheric ozone, their effects on aerosol formation and growth, and their potential influence on global warming. As one of the important BVOC groups, monoterpenes have been a focus of scientific attention in atmospheric research. Detailed regional measurements and model estimates are needed to study emission potential and the monoterpene budget on a global scale. Since the use of empirical measurements for upscaling is limited by many physical and biological factors, such as genetic variation, temperature and light, water availability, seasonal changes, and environmental stresses, comprehensive inventories over larger areas are difficult to obtain. We applied the boundary-layer-chemistry-transport model SOSA (model to Simulate the concentrations of Organic vapours and Sulphuric Acid) to investigate Scots pine (Pinus sylvestris) monoterpene emissions in a boreal coniferous forest at the SMEAR (Station for Measuring forest Ecosystem-Atmosphere Relations) II site, southern Finland. SOSA was applied to simulate monoterpene emissions with three different emission modules: the semiempirical G95, MEGAN (Model of Emissions of Gases and Aerosols from Nature) 2.04 with improved descriptions of temperature and light responses and including also carbonyl emissions, and a process-based model SIM-BIM (Seasonal Isoprenoid synthase Model - Biochemical Isoprenoid biosynthesis Model). For the first time, the emission models included seasonal and diurnal variations in both quantity and chemical species of emitted monoterpenes, based on parameterizations obtained from field measurements. Results indicate that modelling and observations agreed reasonably well and that the model can be used for investigating regional air chemistry questions related to monoterpenes. The predominant modelled monoterpene concentrations, α-pinene and Δ³-carene, are consistent with observations [ABSTRACT FROM AUTHOR]

Over-proportional warming in the northern high latitudes, and large carbon stocks in boreal and (sub)arctic ecosystems have raised concerns as to whether substantial positive climate feedbacks from biogeochemical process responses should be expected. Such feedbacks occur if increasing temperatures lead to e.g., a net release of CO2 or CH4. However, temperature-enhanced emissions of biogenic volatile organic compounds (BVOC) have been shown to contribute to a cooling feedback via growth of secondary organic aerosol (SOA), and related aerosol forcings. Combining measurements in Eastern Siberia with model-based estimates of vegetation and permafrost dynamics, BVOC emissions and aerosol growth, we show here that the additional climate forcing from changes in ecosystem CO2 balance and BVOC-SOA interactions nearly cancel on a regional scale. The interactions between emissions and vegetation dynamics that underlie individual forcing estimates are complex and highlight the importance of addressing ecosystem-climate feedbacks in consistent, process-based model frameworks that account for a multitude of system processes. [ABSTRACT FROM AUTHOR]

Absorption Angstrom exponents (AAE) calculated from filter-based absorption measurements are often used to give information on the origin of the ambient aerosol, for example to distinguish between urban pollution and biomass burning aerosol. Filterbased absorption measurements are a widely used method and are commonly used at aerosol monitoring stations globally. Several correction algorithms are used to account for the artifacts associated with filter-based absorption techniques. These algorithms are of profound importance when determining the absolute amount of absorption by the aerosol. However, this study shows that there are significant differences between the AAEs calculated from these corrections. The study also shows that the difference between AAEs calculated using different corrections can lead to conflicting conclusions on the type of aerosol for the same data set. In this work the AAEs were calculated from data measured with a three-wavelength Particle Soot Absorption Photometer (PSAP) at Elandsfontein on deployed on the South African Highveld for 23 months. The sample air of the PSAP was diluted to prolong filter change intervals. The dilution-corrected PSAP showed a good agreement with a non-diluted MAAP. Thus, the study also shows that the applicability of the PSAP can be extended to remote sites are not often visited or suffer from high levels of pollution. [ABSTRACT FROM AUTHOR]

This work describes improvements in the regional aerosol-climate model REMO-HAM in order to simulate more realistically the process of atmospheric new particle formation (NPF). A new scheme was implemented to simulate OH radical concentrations using a proxy approach based on observations and also accounting for the effects of clouds upon OH concentrations. Second, the nucleation rate calculation was modified to directly simulate the formation rates of 3 nm particles, which removes some unnecessary steps in the formation rate calculations used earlier in the model. Using the updated model version, NPF over Europe was simulated for the periods 2003-2004 and 2008-2009. The statistics of the simulated particle formation events were subsequently compared to observations from 13 ground-based measurement sites. The new model shows improved agreement with the observed NPF rates compared to former versions and can simulate the event statistics realistically for most parts of Europe. [ABSTRACT FROM AUTHOR]

A satellite-based approach to derive the aerosol direct short wave (SW) radiative effect (ADRE) was studied in an environment with highly variable aerosol conditions over Eastern China from March to October 2009. The method is based on using coincident SW Top of the Atmosphere (TOA) fluxes from the Clouds and the Earth's Radiant Energy System (CERES) and aerosol optical depths (AODs) from the Moderate Resolution Imaging Sectroradiometer (MODIS). The estimate for instantaneous clear sky ADRE is obtained by establishing linear regression between CERES fluxes and MODIS AODs. Even though the approach has been used in a number of studies, less focus has been paid to the method itself. In this study the main goals were first to study the method in more detail as well as it's applicability over Eastern China, and second to derive a satellite-based estimate of ADRE over the study area. Before the linear fitting, CERES fluxes were normalized to a fixed solar zenith angle, Earth-Sun distance and atmospheric water vapour content to reduce the noise in the flux observations that was not related to aerosols. The satellite based clear sky estimates for median instantaneous and diurnally averaged ADRE over the study area were -8.8W m-2, and -5.1W m-2, respectively. Over heavily industrialized areas the cooling at TOA was two to more than three times the median value, and associated with high AODs (> 0.5). Especially during the summer months positive ADREs were observed locally over dark surfaces. This was most probably a method artifact related to systematic change of aerosol type, subvisual cloud contamination or both. The key question in the satellite-based approach is the accuracy of the estimated aerosol-free TOA flux (F0,TOA). Comparison with simulated F0,TOA showed that both the satellite method and the model produced qualitatively similar spatial patterns, but absolute values differed. In 58% of the cases the satellite based F0,TOA was within ±10W m-2 of the modeled value. Over bright surfaces the satellite-based method tend to produce lower F0,TOA than the model. [ABSTRACT FROM AUTHOR]

Aerosol effects on low-level clouds over the nordic countries are investigated by combining in situ ground-based aerosol measurements with remote sensing data of clouds and precipitation. Ten years of number size distribution data from two aerosol measurement stations (Vavihill, Sweden and Hyytiälä, Finland) provide aerosol number concentrations in the atmospheric boundary layer. This is combined with cloud satellite data from the Moderate Resolution Imaging Spectroradiometer and weather radar data from the Baltic Sea Experiment. Also, how the meteorological conditions affect the clouds are investigated using reanalysis data from the European Centre for Medium-Range Forecasts. The cloud droplet effective radius is found to decrease when the aerosol number concentration increases, while the cloud optical thickness does not vary with boundary layer aerosol number concentrations. Furthermore, the aerosol cloud interaction parameter (ACI), a measure of how the effective radius is influenced by the number concentration of cloud active particles, is found to be somewhere between 0.10 and 0.18 and the magnitude of the ACI is greatest when the number concentration of particles with a diameter larger than 130 nm is used. Lower precipitation intensity in the weather radar images is associated with higher aerosol number concentrations. In addition, at Hyytiälä the particle number concentrations is generally higher for non-precipitating cases than for precipitating cases. The apparent absence of the first indirect effect of aerosols on low-level clouds over land raises questions regarding the magnitude of the indirect aerosol radiative forcing. [ABSTRACT FROM AUTHOR]